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基于 Mo2C 的 Fe 催化剂中 Fe/Fe 循环的加速促进过一硫酸盐的活化。

Accelerated Fe/Fe cycle in Mo2C-based Fe catalyst to promote peroxymonosulfate activation.

机构信息

National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China.

National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China.

出版信息

Chemosphere. 2024 Nov;367:143380. doi: 10.1016/j.chemosphere.2024.143380. Epub 2024 Sep 20.

DOI:10.1016/j.chemosphere.2024.143380
PMID:39307465
Abstract

The harmful impact of organic pollutants on aquatic ecosystems underscores the pressing need for effective remediation. While activating peroxymonosulfate (PMS) with Fe catalyst offers a promising approach for eliminating these pollutants, its widespread use is hindered by the sluggish regeneration of Fe from Fe. Here, this study demonstrates for the first time that combining an Fe catalyst with MoC (Fe-MoC) enhances the Fe³⁺/Fe⁺ cycle, thereby improving PMS activation. The Fe-MoC/PMS system achieved near-complete degradation of carbamazepine (CBZ) within only 8 min, with an impressive observed rate constant (k) of up to 0.624 min, about 15 times greater than that of Fe-C catalyst. It also exhibits the capability to degrade a broad range of common antibiotics, phenols, and dye-like organic compounds. Through electron paramagnetic resonance (EPR) analysis and quenching experiments, it was verified that hydroxyl radicals (·OH), sulfate radicals (SO), singlet oxygen (O), and superoxide radicals (·O) species during the reaction, with the former three serving as the primary active species. These findings offer a hopeful avenue for the systematic development and enhancement of catalysts specifically designed to efficiently remediate organic pollutants in wastewater.

摘要

有机污染物对水生生态系统的有害影响凸显了有效修复的迫切需要。尽管用铁催化剂激活过一硫酸盐(PMS)为消除这些污染物提供了一种很有前途的方法,但由于从 Fe 中缓慢再生 Fe ,其广泛应用受到阻碍。在此,本研究首次表明,将铁催化剂与 MoC(Fe-MoC)结合可以增强 Fe³⁺/Fe⁺循环,从而提高 PMS 的激活效率。Fe-MoC/PMS 体系仅在 8 分钟内即可实现卡马西平(CBZ)的近乎完全降解,其观察到的速率常数(k)高达 0.624 min⁻¹,是 Fe-C 催化剂的 15 倍以上。它还表现出降解一系列常见抗生素、酚类和类似染料的有机化合物的能力。通过电子顺磁共振(EPR)分析和猝灭实验,验证了反应过程中存在羟基自由基(·OH)、硫酸根自由基(SO)、单线态氧(O)和超氧自由基(·O),其中前三种是主要的活性物质。这些发现为系统地开发和增强专门设计用于有效修复废水中有机污染物的催化剂提供了一个有希望的途径。

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